WO2013128841A1 - プリプレグおよびプリプレグの製造方法 - Google Patents

プリプレグおよびプリプレグの製造方法 Download PDF

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Publication number
WO2013128841A1
WO2013128841A1 PCT/JP2013/000891 JP2013000891W WO2013128841A1 WO 2013128841 A1 WO2013128841 A1 WO 2013128841A1 JP 2013000891 W JP2013000891 W JP 2013000891W WO 2013128841 A1 WO2013128841 A1 WO 2013128841A1
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Prior art keywords
resin
prepreg
resin layer
fiber base
base material
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PCT/JP2013/000891
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English (en)
French (fr)
Japanese (ja)
Inventor
猛 八月朔日
恭史 瀧本
晴行 秦野
亘平 穴田
Original Assignee
住友ベークライト株式会社
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Application filed by 住友ベークライト株式会社 filed Critical 住友ベークライト株式会社
Priority to KR1020147018952A priority Critical patent/KR20140127803A/ko
Publication of WO2013128841A1 publication Critical patent/WO2013128841A1/ja

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    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
    • C08J5/24—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29B—PREPARATION OR PRETREATMENT OF THE MATERIAL TO BE SHAPED; MAKING GRANULES OR PREFORMS; RECOVERY OF PLASTICS OR OTHER CONSTITUENTS OF WASTE MATERIAL CONTAINING PLASTICS
    • B29B15/00—Pretreatment of the material to be shaped, not covered by groups B29B7/00 - B29B13/00
    • B29B15/08—Pretreatment of the material to be shaped, not covered by groups B29B7/00 - B29B13/00 of reinforcements or fillers
    • B29B15/10—Coating or impregnating independently of the moulding or shaping step
    • B29B15/12—Coating or impregnating independently of the moulding or shaping step of reinforcements of indefinite length
    • B29B15/122—Coating or impregnating independently of the moulding or shaping step of reinforcements of indefinite length with a matrix in liquid form, e.g. as melt, solution or latex
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B17/00—Layered products essentially comprising sheet glass, or glass, slag, or like fibres
    • B32B17/02—Layered products essentially comprising sheet glass, or glass, slag, or like fibres in the form of fibres or filaments
    • B32B17/04—Layered products essentially comprising sheet glass, or glass, slag, or like fibres in the form of fibres or filaments bonded with or embedded in a plastic substance
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/12—Layered products comprising a layer of synthetic resin next to a fibrous or filamentary layer
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/18—Layered products comprising a layer of synthetic resin characterised by the use of special additives
    • B32B27/20—Layered products comprising a layer of synthetic resin characterised by the use of special additives using fillers, pigments, thixotroping agents
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/30—Layered products comprising a layer of synthetic resin comprising vinyl (co)polymers; comprising acrylic (co)polymers
    • B32B27/306—Layered products comprising a layer of synthetic resin comprising vinyl (co)polymers; comprising acrylic (co)polymers comprising vinyl acetate or vinyl alcohol (co)polymers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/34—Layered products comprising a layer of synthetic resin comprising polyamides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B27/00—Layered products comprising a layer of synthetic resin
    • B32B27/38—Layered products comprising a layer of synthetic resin comprising epoxy resins
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B5/00—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts
    • B32B5/22—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed
    • B32B5/24—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed one layer being a fibrous or filamentary layer
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/01—Use of inorganic substances as compounding ingredients characterized by their specific function
    • C08K3/013—Fillers, pigments or reinforcing additives
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/34—Silicon-containing compounds
    • C08K3/36—Silica
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K7/00—Use of ingredients characterised by shape
    • C08K7/02—Fibres or whiskers
    • C08K7/04—Fibres or whiskers inorganic
    • C08K7/14—Glass
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/03—Use of materials for the substrate
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/03—Use of materials for the substrate
    • H05K1/0313—Organic insulating material
    • H05K1/0353—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement
    • H05K1/0366—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement reinforced, e.g. by fibres, fabrics
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K3/00—Apparatus or processes for manufacturing printed circuits
    • H05K3/46—Manufacturing multilayer circuits
    • H05K3/4644—Manufacturing multilayer circuits by building the multilayer layer by layer, i.e. build-up multilayer circuits
    • H05K3/4673—Application methods or materials of intermediate insulating layers not specially adapted to any one of the previous methods of adding a circuit layer
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2260/00—Layered product comprising an impregnated, embedded, or bonded layer wherein the layer comprises an impregnation, embedding, or binder material
    • B32B2260/02—Composition of the impregnated, bonded or embedded layer
    • B32B2260/021—Fibrous or filamentary layer
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2260/00—Layered product comprising an impregnated, embedded, or bonded layer wherein the layer comprises an impregnation, embedding, or binder material
    • B32B2260/04—Impregnation, embedding, or binder material
    • B32B2260/046—Synthetic resin
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2262/00—Composition or structural features of fibres which form a fibrous or filamentary layer or are present as additives
    • B32B2262/10—Inorganic fibres
    • B32B2262/101—Glass fibres
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2264/00—Composition or properties of particles which form a particulate layer or are present as additives
    • B32B2264/10—Inorganic particles
    • B32B2264/102—Oxide or hydroxide
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B2457/00—Electrical equipment
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J2300/00—Characterised by the use of unspecified polymers
    • C08J2300/22—Thermoplastic resins
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J2363/00—Characterised by the use of epoxy resins; Derivatives of epoxy resins
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
    • H05K2201/01—Dielectrics
    • H05K2201/0183—Dielectric layers
    • H05K2201/0195—Dielectric or adhesive layers comprising a plurality of layers, e.g. in a multilayer structure
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K2201/00—Indexing scheme relating to printed circuits covered by H05K1/00
    • H05K2201/02—Fillers; Particles; Fibers; Reinforcement materials
    • H05K2201/0275—Fibers and reinforcement materials
    • H05K2201/029—Woven fibrous reinforcement or textile

Definitions

  • the present invention relates to a prepreg and a method for producing the prepreg.
  • Patent Document 1 discloses a prepreg to be applied to a circuit board having such a structure.
  • Patent Document 1 discloses a prepreg in which two resin layers having different thicknesses are formed on both sides of a fiber base material.
  • the present inventors have conceived that these resin layers are composed of different resin compositions so that the resin layer on one side of the prepreg and the resin layer on the other side meet different characteristics.
  • the fiber base material is impregnated with both different resin compositions, it is necessary to make the fiber base material have good impregnation properties, and the design of each resin composition is limited, It has been found that it is difficult to sufficiently achieve the desired characteristics in the layer.
  • the present invention has been invented based on such knowledge.
  • a fiber substrate A first resin layer that covers one surface side of the fiber substrate and is composed of a first resin composition; Covering the other surface side of the fiber substrate, and comprising a second resin layer composed of a second resin composition different from the first resin composition,
  • the second resin layer is provided with a prepreg in which the fiber base material is impregnated over at least 90% of the thickness of the fiber base material from the other surface of the fiber base material.
  • the second resin layer impregnated in the fiber base material is formed at least over 90% of the thickness of the fiber base material from the other surface of the fiber base material. Therefore, it is not necessary to impregnate the fiber base material with a large amount of the first resin layer. Therefore, the 1st resin composition which comprises the 1st resin layer is not restricted to the thing of the good impregnation property with respect to a fiber base material, The breadth of selection of a 1st resin composition spreads. And it can be set as the prepreg provided with the 1st resin layer which has a desired characteristic.
  • the manufacturing method of the prepreg mentioned above can also be provided. That is, according to the present invention, the step of pressure-bonding the first resin sheet to one surface of the fiber substrate to provide the first resin layer made of the first resin composition; Forming a second resin layer made of a second resin composition different from the first resin composition on the other surface side of the fiber substrate, In the step of forming the second resin layer, There is provided a method for producing a prepreg that forms a second resin layer impregnated in the fiber base material over at least 90% of the thickness of the fiber base material from the other surface of the fiber base material.
  • the second resin layer impregnated in the fiber base is formed at least over 90% of the thickness of the fiber base from the other surface of the fiber base. Therefore, it is not necessary to impregnate the fiber base material with a large amount of the first resin sheet. Accordingly, the first resin composition constituting the first resin layer is not limited to the one having good impregnation property to the fiber base material, and the selection range of the first resin composition is widened, and the first resin layer having desired characteristics is provided. Can be formed.
  • a substrate having a cured body of the prepreg described above With a circuit layer, The second resin layer of the cured body of the prepreg embeds the circuit layer, A substrate in which a metal layer is provided on the first resin layer of the cured prepreg can also be provided. Also, with this substrate A semiconductor device including a semiconductor element mounted on the substrate can also be provided.
  • a prepreg and a method for manufacturing a prepreg that have different resin layers and can exhibit the desired characteristics of each resin layer more reliably.
  • FIG. 1 is a view showing a cross section of a prepreg of Example 1.
  • FIG. 6 is a view showing a cross section of a prepreg of Example 5.
  • FIG. 6 is a view showing a cross section of a prepreg of Example 6.
  • FIG. 5 is a view showing a cross section of a prepreg of Comparative Example 1.
  • FIG. 5 is a view showing a cross section of a prepreg of Comparative Example 2.
  • FIG. 1 is a cross-sectional view showing a prepreg.
  • the prepreg 1 of this embodiment is The fiber substrate 2, one surface side of the fiber substrate 2 is coated, the first resin layer 3 composed of the first resin composition, and the other surface side of the fiber substrate 2 are coated,
  • the second resin layer 4 made of a second resin composition different from the one resin composition is provided, the first resin layer 3 and the second resin layer 4 are in contact with each other, and an interface F is formed.
  • the second resin layer 4 is impregnated in the fiber base material 2 over at least 90% of the thickness of the fiber base material 2 from the other surface of the fiber base material 2.
  • the difference between the first resin composition and the second resin composition may be that the types of components constituting each resin composition may be different, or the composition ratio may be different. Good.
  • the manufacturing method of the prepreg of this embodiment includes the step of pressing the first resin sheet 3 ′ on one surface of the fiber substrate 2 to provide the first resin layer 3 made of the first resin composition, and the fiber base. Forming a second resin layer 4 made of a second resin composition different from the first resin composition on the other surface side of the material 2. In the step of forming the second resin layer 4, the second resin layer 4 impregnated in the fiber base material 2 is formed over at least 90% of the thickness of the fiber base material 2 from the other surface of the fiber base material 2. To do.
  • a prepreg 1 shown in FIG. 1 includes a flat fiber substrate 2, a first resin layer 3 positioned on one surface (lower surface) side of the fiber substrate 2, and the other surface (upper surface) of the fiber substrate 2. And a second resin layer 4 located on the side.
  • the prepreg 1 is for a printed wiring board (circuit board).
  • the fiber base material 2 has a function of improving the mechanical strength of the prepreg 1.
  • glass fiber base materials such as glass woven fabric and glass nonwoven fabric, Polyamide resin fibers, polyamide resin fibers such as aramid fibers such as aromatic polyamide resin fibers and wholly aromatic polyamide resin fibers, polyester resin fibers such as polyester resin fibers, aromatic polyester resin fibers, wholly aromatic polyester resin fibers,
  • a synthetic fiber substrate composed of a woven or non-woven fabric mainly composed of at least one of polyparaphenylenebenzobisoxazole, polyimide resin fiber, fluororesin fiber, etc. examples thereof include fiber base materials such as craft paper, cotton linter paper, and organic fiber base materials such as paper fiber base materials mainly composed of linter and kraft pulp mixed paper. Among these, any one or more fiber base materials can be used.
  • the fiber base material 2 is preferably a glass fiber base material.
  • the mechanical strength of the prepreg 1 can be further improved.
  • Examples of the glass constituting such a glass fiber substrate include E glass, C glass, A glass, S glass, D glass, NE glass, T glass, Q glass, H glass, UT glass, and L glass. Any one or more of these can be used. Among these, it is preferable that glass is S glass, T glass, UT glass, or Q glass. Thereby, the thermal expansion coefficient of a glass fiber base material can be made comparatively small, and for this reason, the prepreg 1 can be made as small as possible in the thermal expansion coefficient.
  • the average thickness T of the fiber substrate 2 is not particularly limited, but is preferably 150 ⁇ m or less, more preferably 100 ⁇ m or less, and even more preferably about 10 ⁇ m to 50 ⁇ m.
  • the average thickness T of the fiber base material 2 measured 10 thicknesses from one surface of the fiber base material 2 to the other surface in the intersection part of the warp yarn and the weft of the fiber base material 2, and the average value It is obtained by calculating.
  • the first resin layer 3 is provided on one surface side of the fiber substrate 2, and the second resin layer 4 is provided on the other surface side. Moreover, the 1st resin layer 3 is comprised with the 1st resin composition, and the 2nd resin layer 4 is comprised with the 2nd resin composition different from the said 1st resin composition.
  • the first resin layer 3 covers one surface of the fiber base material 2, and the second resin layer 4 covers the other surface of the fiber base material 2.
  • the first resin layer 3 is a layer on which a wiring part (metal layer) is directly formed.
  • the second resin layer 4 is a layer in which the circuit layer is embedded.
  • the prepreg does not include a film that peels off during the production of the substrate.
  • the first resin layer 3 and the second resin layer 4 are semi-cured (B stage).
  • the 1st resin composition is set to the composition which is excellent in adhesiveness with a metal. More specifically, the 90 ° peel strength A after the first resin layer 3 of the prepreg 1 is superposed on the copper foil and heat-treated in the air under the conditions of load 2 MPa, temperature 220 ° C., 1 hour is The second resin layer 4 of the prepreg 1 is superposed on the copper foil, and is higher than the 90 ° peel strength B after heat treatment in the air under the conditions of a load of 2 MPa, a temperature of 220 ° C. and 1 hour.
  • the peel strength can be measured by peeling the resin layer from the copper foil in the 90-degree direction according to JIS C 6481 90-degree peeling method. Specifically, at 25 ° C., the 90-degree peel strength when the resin layer is peeled off at a speed of 50 mm per minute is measured with a 90-degree peel tester. More specifically, the peel strength A is preferably 0.5 kN / m or more. Furthermore, it is more preferably 0.6 kN / m or more, particularly 0.8 kN / m or more. Adhesiveness with a wiring part can be improved by setting it as 0.5 kN / m or more.
  • the upper limit value of the peel strength A is not particularly limited, but is preferably 2 kN / m or less.
  • the peel strength B is preferably 0.4 N / m or more. Especially, it is preferable that it is 0.5 N / m or more. By setting it to 0.4 N / m or more, adhesion to the inner layer circuit wiring portion can be enhanced.
  • the upper limit value of the peel strength B is not particularly limited, but is preferably 1 kN / m or less.
  • the peel strength A-peel strength B is preferably 0.1 kN / m or more, and more preferably 1.6 kN / m or less.
  • the second resin composition is set so that the second resin layer 4 has a minimum melt viscosity lower than that of the first resin layer 3. It is preferable that The minimum melt viscosity will be described later.
  • the 2nd resin composition which comprises the 2nd resin layer 4 is a composition with the favorable impregnation property to the fiber base material 2. It is preferable that Each resin composition will be described in detail later.
  • the fiber base material 2 is impregnated with a part of the second resin layer 4 over the entire thickness direction.
  • the second resin layer 4 includes an impregnation portion 43 impregnated in the fiber base 2 and a covering portion 42 that covers the surface (the other surface) of the fiber base 2.
  • the impregnation part 43 of the second resin layer 4 impregnates the fiber base material 2 from at least the surface covered with the covering part 42 of the fiber base material 2 to a position of 90% of the thickness of the fiber base material 2.
  • the impregnation part 43 impregnates the fiber base material 2 over the whole thickness of the fiber base material 2.
  • the interface F between the impregnated portion 43 and the first resin layer 3 is located outside the fiber substrate 2. More specifically, the first resin layer 3 is in contact with one surface of the fiber base 2, but is not impregnated inside the fiber base 2. And the impregnation part 43 and the 1st resin layer 3 contact
  • the first resin layer 3 is in direct contact with one surface of the fiber base material 2, but not limited to this, the impregnation portion 43 protrudes from one surface of the fiber base material 2. Thus, the first resin layer 3 may not directly contact one surface of the fiber base 2.
  • the average thickness T of the fiber base 2 is equal to the thickness -ta of the second resin layer 4.
  • the interface of the 1st resin layer 3 and the 2nd resin layer 4 can be confirmed by observing the cross section orthogonal to the thickness direction of the prepreg 1 by SEM.
  • the interface between the first resin layer 3 and the second resin layer 4 is formed over the entire width direction of the prepreg 1.
  • the impregnation part 43 impregnated the fiber base material 2 over the whole thickness of the fiber base material 2 not only this but the 1st resin layer 3 is also in the fiber base material 2. It may be impregnated. As shown in FIG. 2, the impregnation portion 43 of the second resin layer 4 extends from the surface (the other surface) covered with the covering portion 42 of the fiber base material 2 to a position of 90% or more of the thickness of the fiber base material 2.
  • the fiber substrate 2 is impregnated. That is, the thickness ta1 of the impregnated portion 43 is 90% or more of the thickness T of the fiber base 2. Further, the fiber base material 2 is impregnated with the impregnation portion 31 of the first resin layer 3.
  • the impregnation part 31 impregnates the fiber base material 2 from the surface (one surface) of the fiber base material 2 covered with the covering part 32 to a position of 10% or less of the thickness of the fiber base material 2.
  • the thickness tb1 of the impregnation part 31 is 10% or less of the thickness T of the fiber base 2.
  • the impregnation part 31 impregnates a region not impregnated by the impregnation part 43.
  • the 1st impregnation part 31 which is a part of 1st resin layer 3, and the 2nd impregnation part 43 which is a part of 2nd resin layer 4 are located in the fiber base material 2.
  • the 1st impregnation part 31 (lower surface of the 1st resin layer 3) and the 2nd impregnation part 43 (upper surface of the 2nd resin layer 4) are contacting. Further, an interface F is formed at the boundary between the first impregnation portion 31 and the impregnation portion 43.
  • the other points are the same as in FIG.
  • the impregnation part 43 impregnates the fiber base material 2 from the surface covered with the covering part 42 of the fiber base material 2 to a position of 90% or more of the thickness of the fiber base material 2, whereby the second resin The intersection between the interface between the layer 4 and the first resin layer 3 and the fiber substrate 2 can be reduced. Thereby, it can prevent that the metal ion which entered from between the fiber base material 2 and the 2nd resin layer 4 migrates the said interface. Thereby, the insulation reliability between holes can be improved.
  • the impregnation part 31 impregnates the fiber base material 2 from the surface of the fiber base material 2 covered with the covering part 32 to a position of 10% or less of the thickness of the fiber base material 2.
  • the first resin layer 3 may be selected from those having good adhesion to metal, the design range of the first resin layer 3 can be widened.
  • the first resin composition constituting the first resin layer 3 in the fiber base material 2 is obtained by impregnating the woven fiber base material 2 with the first resin layer 3 and the second resin layer 4. It can prevent that the 2nd resin composition which comprises the resin layer 4 gets caught, and peeling arises between the 1st resin layer 3 and the 2nd resin layer 4.
  • the 2nd resin layer 4 has impregnated the fiber base material 2 over the position of 90% of the thickness of the fiber base material 2 as follows.
  • the average value T of the thickness of the fiber base material 2 is calculated, and 90% of this thickness is calculated (numerical value C).
  • the average value D (10 places measurement) of the distance from the other surface of the fiber base material 2 to the interface F of the 1st resin layer 3 and the 2nd resin layer 4 should just exceed the numerical value C.
  • the minimum melt viscosity (eta) 1 of the 1st resin layer 3, the 2nd resin layer 4 is mentioned, for example.
  • the ratio ( ⁇ 1 / ⁇ 2) of the minimum melt viscosity ⁇ 2 is 1.1 times or more, and at the time of production, one of the layers is supplied to the fiber substrate 2 in the form of a sheet, and the other layer is varnished to form fibers. What is necessary is just to supply to the base material 2.
  • the average thickness of the covering portion 42 of the second resin layer 4 and t a [ ⁇ m], among the first resin layer 3, the average thickness of the portion covering the one surface of the fiber substrate 2 t b [[mu] m] and the time, t a is preferably larger than t b.
  • a wiring part can be formed on the surface of the prepreg 1 (on the resin layer 3) with high workability.
  • the second resin layer 4 can have high flexibility and sufficient thickness, when embedding the wiring portion of another prepreg 1 or another fiber base material in the second resin layer 4, The embedding can be performed reliably, that is, the embedding property to the wiring part of other prepreg 1 and other fiber base material is improved.
  • the average thickness t b is preferably 0.1 to 15 ⁇ m, and more preferably 1 to 10 ⁇ m.
  • the average thickness t a is preferably from 4 ⁇ 50 [mu] m, and more preferably 8 ⁇ 40 [mu] m.
  • the average thickness t a and the average thickness t b is measured 10 points at arbitrary intervals, obtained by calculating the average value.
  • the minimum melt viscosity ( ⁇ 1) of the first resin layer 3 and the minimum melt viscosity ( ⁇ 2) of the second resin layer 4 in the range of 50 to 150 ° C. when the temperature is increased from 25 ° C. at a rate of 3 ° C./min. ) 1 / ⁇ 2 is preferably 1.1 or more and 100 or less.
  • the minimum melt viscosity ( ⁇ 1) of the first resin layer 3 is higher than the minimum melt viscosity ( ⁇ 2) of the second resin layer 4.
  • the first resin layer 3 and the second resin layer 4 are not mixed, and the interface between the first resin layer 3 and the second resin layer 4 is achieved. Can be formed. Moreover, there exists an effect of improving the adhesiveness of an interface by making minimum melt viscosity ratio (eta) 1 / (eta) 2 into 100 or less, especially 80 or less.
  • the measurement conditions for the minimum melt viscosity are as follows. Using a dynamic viscoelasticity measuring device, measurement is performed under the conditions of a measurement frequency of 62.83 rad / sec, a temperature rising rate of 3 ° C./min, and 50 to 150 ° C.
  • the minimum melt viscosity ⁇ 1 of the first resin layer 3 is preferably 1000 Pa ⁇ s or more and 25000 Pa ⁇ s or less.
  • the minimum melt viscosity ( ⁇ 2) of the second resin layer 4 is preferably 50 Pa ⁇ s or more and 10000 Pa ⁇ s or less, more preferably 5000 Pa ⁇ s or less, and further 3000 Pa ⁇ s or less. desirable.
  • the minimum melt viscosity ( ⁇ 1) of the first resin layer 3 is 1.1 times or more the minimum melt viscosity ( ⁇ 2) of the second resin layer 4, and the minimum melt viscosity of each resin layer is in the above-described range.
  • the prepreg 1 of this embodiment also satisfies the following characteristics.
  • the resin flow measured by heating and pressurizing for 5 minutes under the conditions of 171 ⁇ 3 ° C. and 1380 ⁇ 70 kPa is 15 wt% or more and 50 wt% or less,
  • the prepreg 1 is sandwiched between a pair of opposing rubber plates and heated and pressurized under the conditions of 120 ° C.
  • the weight of the resin layer protruding from the outer edge of the fiber substrate 2 in plan view (first 1 resin layer 3 and the total weight of the second resin layer 4) is 5% or less with respect to the total weight of the entire first resin layer 3 and the entire second resin layer 4, and the rubber plate is the following (i) Satisfy (iii). (I) Rubber hardness measured in accordance with JIS K 6253 A is 60 ° (Ii) Thickness 3mm (Iii) Material is silicon
  • the resin flow measured by heating and pressurizing for 5 minutes under the conditions of 171 ⁇ 3 ° C. and 1380 ⁇ 70 kPa is 15% by weight or more.
  • a prepreg excellent in embedding property can be obtained.
  • the upper limit of the resin flow is 50% by weight or less, the outflow of the resin layer from the prepreg can be suppressed when the prepreg is laminated and pressed. Therefore, when it is laminated on a core layer (see FIG. 5) such as the inner layer circuit board 13, the build-up is excellent in embedding of the circuit of the inner layer circuit board 13 and can suppress the outflow of the resin layer from the prepreg during the lamination press.
  • a core layer see FIG. 5
  • the build-up is excellent in embedding of the circuit of the inner layer circuit board 13 and can suppress the outflow of the resin layer from the prepreg during the lamination press.
  • the weight of the resin layer protruding from the outer edge of the fiber substrate 2 in plan view is 5
  • the thickness uniformity of the obtained laminated board can be improved by setting it as the weight% or less. Therefore, when laminated on the inner layer circuit board 13, the prepreg has excellent circuit embedding properties, can suppress the outflow of the resin layer from the prepreg during the lamination press, and can improve the thickness uniformity. Becomes feasible.
  • the lower limit of the weight of the resin layer protruding from the outer edge of the fiber substrate 2 in plan view when heated and pressurized under the conditions of 120 ° C. and 2.5 MPa with the prepreg 1 sandwiched between a pair of opposing rubber plates Although a value is not specifically limited, For example, it is 0.1 weight%.
  • the first resin composition and the second resin composition preferably have the following compositions.
  • the first resin composition includes, for example, a thermosetting resin, and includes at least one of a curing aid (for example, a curing agent and a curing accelerator) and an inorganic filler as necessary. .
  • a curing aid for example, a curing agent and a curing accelerator
  • an inorganic filler as necessary.
  • thermosetting resin having excellent adhesion with the metal for example, curing agent, curing acceleration
  • curing aid for example, curing agent, curing acceleration
  • a method using an acid-soluble material as an inorganic filler for example, curing agent, curing acceleration
  • a method using an inorganic filler and an organic filler in combination for example, a method using a specific thermoplastic resin, and the like.
  • thermosetting resins examples include urea (urea) resins, melamine resins, bismaleimide resins, polyurethane resins, resins having a benzoxazine ring, cyanate ester resins, bisphenol S type epoxy resins, bisphenol F type epoxy resins, and bisphenols.
  • An epoxy resin such as a copolymerized epoxy resin of S and bisphenol F is preferably used. Any one or more of these can be used. Of these, it is particularly preferable to use a cyanate resin (including a prepolymer of cyanate resin) as the thermosetting resin.
  • Such a cyanate resin can be obtained, for example, by reacting a cyanogen halide with a phenol and prepolymerizing it by a method such as heating, if necessary.
  • cyanate resins include novolak-type cyanate resins, bisphenol A-type cyanate resins, bisphenol E-type cyanate resins, and tetramethylbisphenol F-type cyanate resins. Any one or more of these can be used. Among these, it is preferable that cyanate resin is a novolak-type cyanate resin.
  • the cross-link density increases in the first resin layer 3 after curing after the substrate 10 (see FIG. 5) described later is manufactured, so that the first resin layer 3 (obtained after curing) is obtained.
  • the heat resistance and flame retardancy of the substrate) can be improved.
  • the improvement in heat resistance is thought to be due to the fact that the novolac-type cyanate resin forms a triazine ring after the curing reaction.
  • the flame retardancy is improved because the novolak-type cyanate resin has a high proportion of benzene rings due to its structure, so that the benzene rings are easily carbonized (graphitized), and the first resin layer 3 after curing has carbonized portions. It is thought that it originates in what happens.
  • a novolac-type cyanate resin is used, even if the prepreg 1 is thinned (for example, 35 ⁇ m or less in thickness), excellent rigidity can be imparted to the prepreg 1. Moreover, since the cured product is excellent in rigidity at the time of heating, the obtained substrate 10 is also excellent in reliability when the semiconductor element 500 (see FIG. 6) is mounted. Specifically, a novolac type cyanate resin represented by the formula (I) can be used.
  • the average number of repeating units “n” is not particularly limited, but is preferably 1 to 10, and more preferably 2 to 7.
  • the average number of repeating units “n” is less than the lower limit, the novolac cyanate resin is easily crystallized, and thus the solubility in a general-purpose solvent decreases. For this reason, the first resin composition may be difficult to handle depending on the content of the novolac-type cyanate resin.
  • thermosetting resin for example, novolak type such as phenol novolak resin, cresol novolak resin, bisphenol A novolak resin, etc.
  • thermosetting such as epoxy resin, novolak epoxy resin, cresol novolak epoxy resin such as cresol novolak epoxy resin, epoxy resin such as biphenyl type epoxy resin, unsaturated polyester resin, diallyl phthalate resin, silicone resin It is also possible to use fat. Any one or more of these can be used.
  • the content of the thermosetting resin is not particularly limited, but is preferably 5 to 50% by weight, more preferably 10 to 40% by weight, based on the entire first resin composition.
  • the content of the thermosetting resin is less than the lower limit, depending on the type of the thermosetting resin, the viscosity of the varnish of the first resin composition becomes too low, and it becomes difficult to form the prepreg 1. There is a case.
  • the content of the thermosetting resin exceeds the upper limit, the amount of other components is too small, and the mechanical strength of the prepreg 1 may decrease depending on the type of the thermosetting resin.
  • it says a resin composition it means what remove
  • Examples of the above-described curing aid include tertiary amines such as triethylamine, tributylamine, diazabicyclo [2,2,2] octane, 2-ethyl-4-ethylimidazole, 2-phenyl-4-methylimidazole, 2-phenyl-4-methyl-5-hydroxymethylimidazole, 2-phenyl-4,5-dihydroxymethylimidazole, 2,4-diamino-6- [2'-methyl Imidazolyl- (1 ′)]-ethyl-s-triazine, 2,4-diamino-6- (2′-undecylimidazolyl) -ethyl-s-triazine, 2,4-diamino-6- [2′-ethyl Imidazole compounds such as -4-methylimidazolyl- (1 ′)]-ethyl-s
  • the curing aid is selected from imidazole compounds having two or more functional groups selected from an aliphatic hydrocarbon group, an aromatic hydrocarbon group, a hydroxyalkyl group, and a cyanoalkyl group.
  • 2-phenyl-4,5-dihydroxymethylimidazole is more preferable.
  • Examples of the first resin composition include organic metal salts such as zinc naphthenate, cobalt naphthenate, tin octylate, cobalt octylate, bisacetylacetonate cobalt (II), and trisacetylacetonate cobalt (III). Further, phenol compounds such as phenol, bisphenol A and nonylphenol, organic acids such as acetic acid, benzoic acid, salicylic acid and paratoluenesulfonic acid can be used in combination. Any one or more of these can be used.
  • the content thereof is preferably 0.01 to 3% by weight, more preferably 0.1 to 1% by weight, based on the entire first resin composition.
  • the first resin composition preferably contains an inorganic filler.
  • the inorganic filler examples include talc, alumina, glass, silica such as fused silica, mica, aluminum hydroxide, magnesium hydroxide, and the like. Any one or more of these can be used. Further, depending on the purpose of use of the inorganic filler, a crushed or spherical one is appropriately selected. Among these, from the viewpoint of excellent low thermal expansibility, the inorganic filler is preferably silica, and more preferably fused silica (particularly spherical fused silica).
  • the average particle size of the inorganic filler is preferably 0.01 to 5.0 ⁇ m, and more preferably 0.2 to 2.0 ⁇ m.
  • the average particle size is d 50, can be measured as follows.
  • the inorganic filler is dispersed in water by ultrasonic waves, and the particle size distribution of the inorganic filler is measured on a volume basis by a dynamic light scattering particle size distribution measuring device (LB-550, manufactured by HORIBA). The median diameter is averaged. The particle diameter was taken.
  • spherical fused silica having an average particle size of 5.0 ⁇ m or less is preferable.
  • an acid-soluble inorganic filler may be used as the inorganic filler.
  • the adhesion (plating adhesion) of the wiring part to the first resin layer 3 can be improved.
  • the acid-soluble inorganic filler include metal oxides such as calcium carbonate, zinc oxide, and iron oxide.
  • an inorganic filler and an organic filler may be used in combination.
  • the organic filler include resin fillers such as liquid crystal polymer and polyimide.
  • the content thereof is not particularly limited, but is preferably 20 to 70% by weight, more preferably 30 to 60% by weight of the entire first resin composition.
  • a cyanate resin particularly a novolac-type cyanate resin
  • an epoxy resin substantially free of halogen atoms
  • the epoxy resin include phenol novolac type epoxy resin, bisphenol type epoxy resin, naphthalene type epoxy resin, arylalkylene type epoxy resin, and the like. Any one or more of these can be used.
  • the epoxy resin is preferably at least one of a naphthalene type epoxy resin and an arylalkylene type epoxy resin.
  • the naphthalene type epoxy resin means one having a naphthalene skeleton in a repeating unit.
  • a naphthol type epoxy resin, a naphthalene diol type epoxy resin, a bifunctional to tetrafunctional epoxy type naphthalene resin, a naphthylene ether type epoxy resin and the like are preferable. Any one or more of these can be used. Thereby, heat resistance and low thermal expansibility can further be improved.
  • the naphthalene ring has a higher ⁇ - ⁇ stacking effect than the benzene ring, it is particularly excellent in low thermal expansion and low thermal shrinkage.
  • the polycyclic structure has a high rigidity effect and the glass transition temperature is particularly high, the change in heat shrinkage before and after reflow is small.
  • the naphthol type epoxy resin for example, the following general formula (VII-1); as the naphthalene diol type epoxy resin, the following formula (VII-2); as the bifunctional or tetrafunctional epoxy type naphthalene resin, the following formula (VII-3):
  • Examples of (VII-4) (VII-5) and naphthylene ether type epoxy resins can be represented by the following general formula (VII-6), and one or more of these can be used.
  • naphthylene ether type epoxy resins are preferred from the viewpoint of low water absorption and low thermal expansion.
  • the naphthylene ether type epoxy resin is an epoxy resin having a structure in which a naphthalene skeleton is bonded to another arylene structure via an oxygen atom.
  • N represents an average of 1 to 6 and R represents a glycidyl group or a hydrocarbon group having 1 to 10 carbon atoms, provided that one of R is a glycidyl group.
  • R 1 represents a hydrogen atom or a methyl group
  • R 2 each independently represents a hydrogen atom, an alkyl group having 1 to 4 carbon atoms, an aralkyl group, a naphthalene group, or a glycidyl ether group-containing naphthalene.
  • o and m are each an integer of 0 to 2, and either o or m is 1 or more.
  • naphthylene ether type epoxy resin for example, those represented by the following formulas (6) and (7) may be used.
  • the arylalkylene type epoxy resin refers to an epoxy resin having one or more arylalkylene groups in a repeating unit, and examples thereof include a xylylene type epoxy resin and a biphenyldimethylene type epoxy resin. Any one or more of these can be used. Among these, the aryl alkylene type epoxy resin is preferably a biphenyl dimethylene type epoxy resin.
  • biphenyl dimethylene type epoxy resin represented by the formula (II) can be used.
  • the average number of repeating units “n” of the biphenyldimethylene type epoxy resin represented by the formula (II) is not particularly limited, but is preferably 1 to 10, and more preferably 2 to 5.
  • the average number of repeating units “n” is less than the lower limit, the biphenyldimethylene type epoxy resin is easily crystallized, so that the solubility in a general-purpose solvent decreases. For this reason, the varnish of the first resin composition may be difficult to handle.
  • the average number of repeating units “n” exceeds the upper limit, depending on the solvent used, the viscosity of the varnish of the first resin composition may increase. In this case, the fiber base material 2 cannot be sufficiently impregnated with the first resin composition, and as a result, molding failure of the prepreg 1 and mechanical strength may be reduced.
  • the lower limit of the content of the epoxy resin is not particularly limited, but is preferably 1% by weight or more, and particularly preferably 2% by weight or more in the entire resin composition. If the content is too small, the reactivity of the cyanate resin may decrease, or the moisture resistance of the resulting product may decrease. Although the upper limit of content of an epoxy resin is not specifically limited, 40 weight% or less is preferable. If the content is too large, the heat resistance may decrease.
  • the lower limit of the weight average molecular weight (Mw) of the epoxy resin is not particularly limited, but is preferably 500 or more, more preferably 800 or more. If Mw is too small, tackiness may occur in the resin layer.
  • the upper limit of Mw is not particularly limited, but is preferably Mw 20,000 or less, and particularly preferably Mw 15,000 or less. If Mw is too large, the impregnation property to the fiber base material may be deteriorated during the production of the insulating resin layer, and a uniform product may not be obtained.
  • the Mw of the epoxy resin can be measured by GPC, for example.
  • a resin etc. which improves adhesiveness with a metal.
  • examples of such components include thermoplastic resins such as phenoxy resins, polyvinyl acetal resins, and polyamide resins, and it is preferable to include any one or more of these.
  • these resins it is preferable to include a phenoxy resin from the viewpoint of adhesion to a metal.
  • the first resin composition preferably contains a coupling agent.
  • phenoxy resin examples include a phenoxy resin having a bisphenol skeleton, a phenoxy resin having a naphthalene skeleton, and a phenoxy resin having a biphenyl skeleton.
  • a phenoxy resin having a structure having a plurality of these skeletons can also be used. Any one or more of these may be used as the phenoxy resin.
  • a phenoxy resin having a biphenyl skeleton and a bisphenol S skeleton as the phenoxy resin. Accordingly, the glass transition temperature of the phenoxy resin can be increased due to the rigidity of the biphenyl skeleton, and the adhesion of the phenoxy resin to the metal can be improved due to the presence of the bisphenol S skeleton. As a result, the heat resistance of the first resin layer 3 can be improved, and the adhesion of the wiring part (metal) to the first resin layer 3 can be improved when a multilayer substrate is manufactured.
  • a phenoxy resin having a bisphenol A skeleton and a bisphenol F skeleton as the phenoxy resin.
  • the adhesiveness to the 1st resin layer 3 of a wiring part can further be improved at the time of manufacture of a multilayer substrate.
  • the molecular weight of the phenoxy resin is not particularly limited, but the weight average molecular weight is preferably 5,000 to 70,000, more preferably 10,000 to 60,000.
  • the phenoxy resin When the phenoxy resin is used, its content is not particularly limited, but it is preferably 1 to 40% by weight, more preferably 5 to 30% by weight of the entire first resin composition.
  • the polyvinyl acetal resin is a resin obtained by acetalizing polyvinyl alcohol with a carbonyl compound such as formaldehyde or acetaldehyde.
  • examples of the polyvinyl acetal resin include polyvinyl formal and polyvinyl butyral. Any one or more of these can be used.
  • the degree of acetalization of the polyvinyl acetal resin is preferably 40% or more from the viewpoint of water absorption and 80% or less from the viewpoint of compatibility.
  • the polyamide-based resin include aromatic polyamides from the viewpoint of heat resistance.
  • a weight average molecular weight of a polyamide-type resin is 15,000 or more from an adhesive viewpoint with a conductor layer.
  • polyamide-based resin examples include phenolic hydroxyl group-containing aromatic polyamide-poly (butadiene-acrylonitrile) block copolymers (for example, trade name KAYAFLEX BPAM-155 (Nippon Kayaku, terminal is an amide group)).
  • thermoplastic resin as described above is preferably 1 to 40% by weight, more preferably 10 to 30% by weight, based on the entire first resin composition.
  • the coupling agent it is preferable to use at least one selected from, for example, an epoxy silane coupling agent, a titanate coupling agent, an aminosilane coupling agent, and a silicone oil type coupling agent.
  • the coupling agent When the coupling agent is used, its content is not particularly limited, but it is preferably 0.05 to 3 parts by weight, more preferably 0.1 to 2 parts by weight with respect to 100 parts by weight of the inorganic filler. More preferred.
  • the first resin composition can contain additives such as an antifoaming agent, a leveling agent, a pigment, and an antioxidant as necessary.
  • the second resin composition has a composition different from that of the first resin composition. Specifically, the second resin layer 4 has a better embedding property than the first resin layer 3 and further has a composition satisfying the above-described physical properties. Has been.
  • the constituents of the second resin composition can be the same as those mentioned in the first resin composition, but the type and content of the resin and filler, the molecular weight of the resin (average number of repeating units) ) Etc. are different. As a result, the second resin layer 4 has different characteristics from the first resin layer 3.
  • the 2nd resin composition contains the thermoplastic resin mentioned above, a thermosetting resin, an inorganic filler, a hardening accelerator etc., for example.
  • the second resin composition includes, for example, the above-described epoxy resin, cyanate resin, and inorganic filler.
  • the epoxy resin an epoxy resin having the above-described naphthalene skeleton and a structure in which the naphthalene skeleton is bonded to another arylene structure via an oxygen atom is preferable.
  • the inorganic filler contained in the second resin layer 4 is preferably spherical fused silica having an average particle diameter of 5.0 ⁇ m or less, and preferably has an average particle diameter of 0.01 to 2.0 ⁇ m, particularly an average particle diameter of 10 to 50 nm. Spherical fused silica is more preferred.
  • the heat resistance of the prepreg 1 can be improved by using such silica (nanosilica) having an average particle size of 50 nm or less.
  • the second resin composition preferably contains silica having an average particle diameter of 0.5 to 5 ⁇ m in addition to the silica having a particle diameter of 50 nm or less.
  • the first resin composition preferably uses silica having an average particle size of 0.5 ⁇ m to 50 nm in order to form fine irregularities and improve the adhesion to the conductor circuit layer.
  • the content of the thermoplastic resin in the second resin layer 4 is lower than the content of the thermoplastic resin in the first resin layer 3. By doing in this way, the embedding property of the circuit of the 2nd resin layer 4 can be improved.
  • the adhesiveness of the conductor circuit in the 1st resin layer 3 can be made favorable.
  • the content of the thermoplastic resin in the second resin layer 4 is preferably 10% by weight or less, more preferably 5% by weight or less of the second resin composition constituting the second resin layer 4. .
  • the second resin layer 4 may not include a thermoplastic resin.
  • the prepreg 1 as described above can be manufactured as follows using the manufacturing apparatus shown in FIG. As shown in FIG. 3, the manufacturing apparatus 6 includes rollers 621 to 628, a nozzle (a die coater that is a discharge means) 611, and a drying device 64.
  • the manufacturing apparatus 6 includes rollers 621 to 628, a nozzle (a die coater that is a discharge means) 611, and a drying device 64.
  • the roller 621 is a means for sending out a first resin sheet 3 ′ to be the first resin layer 3.
  • the roller 621 includes a first resin sheet 3 ′ with a support 51 (in FIG. 3, the support 51 and the first resin sheet 3 ').
  • a sheet composed of one resin sheet 3 ′ is referred to as a sheet 5).
  • the roller 621 is configured to rotate by a motor (drive source) (not shown). When the roller 621 rotates, the sheet 5 including the first resin sheet 3 ′ is sent out from the roller 621.
  • a motor drive source
  • metal foil metal foil
  • a metal foil is a part processed into a wiring part (circuit) etc., for example.
  • the metal material constituting the metal foil examples include copper or a copper-based alloy, aluminum or an aluminum-based alloy, iron or an iron-based alloy, and stainless steel. And among these, as a metal material which comprises metal foil, it is excellent in electroconductivity, the circuit formation by an etching is easy, and since it is cheap, copper or a copper-type alloy is preferable.
  • the minimum melt viscosity at 50 to 150 ° C. of the first resin sheet 3 ′ is 1000 Pa ⁇ s or more and 25000 Pa ⁇ s or less. As described above, when the minimum melt viscosity at 50 to 150 ° C. is set to 1000 Pa ⁇ s or more, the first resin sheet 3 ′ is less likely to be impregnated into the fiber substrate 2. Moreover, it becomes difficult to mix with the second resin layer 4. By setting the minimum melt viscosity at 50 to 150 ° C. to 25000 Pa ⁇ s or less, adhesion to the fiber base material 2 can be secured. The measuring method is as described above.
  • the roller 623 is a means for feeding out the fiber base material 2, and the fiber base material 2 is wound around the roller 623.
  • the roller 623 is configured to rotate by a motor (not shown), and when the roller 623 rotates, the fiber base material 2 is continuously sent out from the roller 623.
  • roller 622 is a means for regulating the moving direction of the sheet 5, and is installed at the subsequent stage of the roller 621.
  • roller 624 is a means for regulating the moving direction of the fiber base material 2 and is installed at the rear stage of the roller 622.
  • the roller 625 is a means for bonding the first resin sheet 3 ′ and the fiber base material 2, and is installed at the subsequent stage of the rollers 622 and 624.
  • the first resin sheet 3 ′ is conveyed along the outer peripheral surface of the roller 625 so as to contact the outer peripheral surface.
  • the first resin sheet 3 ′ is in surface contact with the quarter of the circumference of the roller 625 through the support 51.
  • the fiber base material 2 is also conveyed along the outer peripheral surface of the roller 625 so as to contact the outer peripheral surface.
  • the fiber base 2 comes into contact with the roller 625 through the first resin sheet 3 ′ where the roller 625 is in indirect contact with the first resin sheet 3 ′.
  • the fiber base material 2 is conveyed along the outer peripheral surface of the roller 625 so as to contact the outer peripheral surface.
  • the contact area between the fiber base 2 and the roller 625 is smaller than the contact area between the first resin sheet 3 ′ and the roller 625.
  • the fiber base 2 and the first resin sheet 3 ′ are pulled in the transport direction, and tension is applied to them.
  • the 1st resin sheet 3 'and the fiber base material 2 can be crimped
  • the rollers 626 and 627 are means for regulating the moving direction of the sheet 5 including the first resin sheet 3 ′, the fiber base 2, and the second resin layer 4 on the fiber base 2. They are installed in the order after 625.
  • the roller 628 is a means for winding the prepreg 1.
  • the roller 628 is configured to rotate by a motor (not shown). When the roller 628 rotates, the prepreg 1 is wound around the roller 628.
  • the nozzle 611 discharges (supplies) a liquid (varnish-like) second resin composition at normal temperature (25 ° C.) on the surface of the fiber base 2 opposite to the first resin layer 3 (for example, Die coater).
  • a liquid varnish-like second resin composition at normal temperature (25 ° C.) on the surface of the fiber base 2 opposite to the first resin layer 3 (for example, Die coater).
  • liquid is not limited to liquid but is a concept that includes fluidity.
  • the drying device 64 is installed between the nozzle 611 and the roller 626.
  • a device that performs drying while horizontally conveying an object is used. Thereby, the tension
  • the first resin sheet 3 ′ is in the B stage state. Next, in the roller 625, the first resin sheet 3 ′ and the fiber base material 2 are pressure-bonded.
  • the angle (bonding angle) ⁇ between the first resin sheet 3 ′ and the fiber base material 2 at this time is preferably an acute angle. Thereby, it can prevent or suppress that distortion arises in the fiber base material 2.
  • tensile_strength by the side of the fiber base material 2 is smaller than the tension
  • the tension on the fiber base 2 side is preferably 30 N or less, and more preferably about 15 to 25 N. Thereby, the dimensional change and internal distortion of the fiber base material 2 can be prevented or suppressed.
  • tensile_strength of 1st resin sheet 3 ' is adjusted and a 1st resin layer is made into the fiber base material 2. As shown in FIG. Can be impregnated.
  • the varnish containing 1st resin sheet 3 'and 2nd resin composition is heat-dried with the drying apparatus 64.
  • FIG. Thereby, the prepreg 1 is obtained.
  • the prepreg 1 is wound around a roller 628.
  • the 1st resin layer can be impregnated in the fiber base material 2 also in this drying process.
  • the drying conditions are not particularly limited, and are appropriately set according to the composition of the first resin composition and the second resin composition (particularly the composition of the second resin composition) and various conditions, but the second resin composition It is preferable to set the volatile component in the product to be 1.5 wt% or less with respect to the resin, and it is more preferable to set it to be about 0.8 to 1.0 wt%.
  • the drying temperature is preferably 100 to 150 ° C., more preferably about 100 to 130 ° C.
  • the drying time is preferably about 2 to 10 minutes, more preferably about 2 to 5 minutes.
  • the first resin sheet 3 ′ is pressure-bonded to the fiber base 2, while the varnish containing the second resin composition is supplied to the fiber base 2 when forming the second resin layer 4. ing.
  • the interface between the 1st resin layer 3 and the 2nd resin layer 4 can be formed reliably.
  • the varnish containing a 2nd resin composition is supplied to the fiber base material 2, it is easy to make the fiber base material 2 impregnate a 2nd resin composition.
  • the first resin layer 3 is formed into a sheet shape in advance and is supplied to the fiber base material 2 in a sheet shape. It has become. Thereby, the prepreg 1 which the 2nd resin layer 4 impregnated the fiber base material 2 over the position of 90% of the thickness of the fiber base material 2 can be manufactured easily.
  • the prepreg 1 is manufactured by using the manufacturing apparatus 6 shown in FIG. 3, but the prepreg 1 can also be manufactured by using the manufacturing apparatus 6a shown in FIG.
  • the manufacturing apparatus 6 a does not include the nozzle 611 of the manufacturing apparatus 6 but includes a bonding apparatus 65 and a roller 629. The other points are the same as the manufacturing apparatus 6.
  • the laminating device 65 is installed between the roller 627 and the roller 628.
  • the laminating device 65 has a pair of rollers 651 and 652 arranged opposite to each other and a heating unit (not shown) that heats the rollers 651 and 652, and sandwiches an object between the rollers 651 and 652,
  • the object is configured to be pressurized and heated.
  • the roller 629 is installed in the front stage of the bonding apparatus 65.
  • the roller 629 is a means for feeding an object, and a sheet 7 described later is wound around the roller 629.
  • the roller 629 is configured to be rotated by a motor (not shown). When the roller 629 rotates, the sheet 7 is continuously fed out from the roller 629.
  • the drying device 64 In the drying device 64, the fiber base 2 and the first resin sheet 3 ′ are heated, and the first resin sheet 3 ′ is melted. In addition, when not impregnating the fiber base material 2 with the 1st resin layer 3 like FIG. 1, the drying apparatus 64 does not need to be.
  • the roller 629 of the manufacturing apparatus 6a is rotated, and the sheet 7 is sent out from the roller 629. As shown in FIG. 4, the sheet 7 includes a resin film 8 and a second resin sheet 4 ′ provided on one surface of the resin film 8 and made of a solid or semi-solid second resin composition. Have.
  • the second resin sheet 4 ′ is in a B stage state.
  • the second resin sheet 4 ′ is lower than the minimum melt viscosity ( ⁇ 1) at 50 to 150 ° C. of the first resin sheet 3 ′.
  • the second resin sheet 4 ′ can be easily impregnated into the fiber base material 2, and the second resin layer 4 can be impregnated up to 90% or more of the thickness of the fiber material 2.
  • the minimum melt viscosity ratio ⁇ 1 / ⁇ 2 to 1.1 or more, the first resin layer 3 and the second resin layer 4 are not mixed, and the interface between the first resin layer 3 and the second resin layer 4 is achieved. Can be formed.
  • the lowest melt viscosity ( ⁇ 1) of the first resin sheet 3 ′ is preferably 1000 Pa ⁇ s or more and 25000 Pa ⁇ s or less.
  • the minimum melt viscosity ( ⁇ 2) of the second resin sheet 4 ′ is preferably 50 Pa ⁇ s or more and 10000 Pa ⁇ s or less, more preferably 5000 Pa ⁇ s or less, and further 3000 Pa ⁇ s or less. Is desirable.
  • the measuring method is as described above.
  • the same film as that described as the resin film of the support 51 can be used.
  • the sheet 7 and the sheet 5 that is a laminate of the fiber base material 2 and the support 51 pass between the roller 651 and the roller 652 of the laminating device 65,
  • the laminated body of the fiber base material 2 and the support 51 is pressurized and heated by the laminating device 65.
  • seat 7 is crimped
  • the prepreg 1 is wound around a roller 628.
  • the conditions at the time of the pressure bonding are not particularly limited, and are appropriately set according to the composition and various conditions of the second resin composition of the second resin layer 4, but the pressure is 0.1 to 1.0 MPa / cm. preferably 2 mm, more preferably 0.3 ⁇ 0.5 MPa / cm 2 or so.
  • the heating temperature is preferably 100 to 130 ° C.
  • the first resin sheet 3 ′ and the second resin sheet 4 ′ are melted by heating at the time of the pressure bonding, but by keeping the minimum melt viscosity of the second resin layer 4 lower than that of the first resin layer 3,
  • the second resin layer 4 can be impregnated into the fiber substrate 2. Further, as described above, the minimum melt viscosity ratio ⁇ 1 / ⁇ 2 between the first resin layer 3 and the second resin layer 4 is set to 1.1 or more, so that the first resin layer 3 and the second resin layer 4 An interface can be formed between them.
  • a substrate 10 shown in FIG. 5 includes a laminate 11 and metal layers 12 provided on both surfaces of the laminate 11.
  • the laminated body 11 includes two prepregs 1 arranged with the second resin layers 4 facing each other, and an inner layer circuit board 13 sandwiched between the second resin layers 4.
  • the resin layers 3 and 4 of the prepreg 1 are completely cured on the substrate.
  • the circuit layer (not shown) formed on the surface of the inner layer circuit board 13 is securely embedded in the second resin layer 4.
  • the metal layer 12 is a part that is processed into a wiring part, for example, by bonding a metal foil such as a copper foil or an aluminum foil to the laminate 11, or plating copper or aluminum on the surface of the laminate 11. It is formed. Moreover, the support body 51 mentioned above can also be used as the metal layer 12.
  • the peel strength between the metal layer 12 and the first resin layer 3 is preferably 0.5 kN / m or more, and more preferably 0.6 kN / m or more. Thereby, the connection reliability in the semiconductor device 100 (refer FIG. 6) obtained by processing the metal layer 12 into a wiring part can be improved more.
  • Such a substrate 10 is prepared by preparing two prepregs 1 in which a metal layer 12 is formed on the first resin layer 3 and sandwiching the inner layer circuit board 13 between these prepregs 1, for example, in a vacuum press, normal pressure, etc.
  • a laminator and a method of laminating using a laminator that is heated and pressurized under vacuum are exemplified.
  • the vacuum press can be performed with a normal hot press machine or the like sandwiched between flat plates.
  • a vacuum press manufactured by Meiki Seisakusho Co., Ltd. a vacuum press manufactured by Kitagawa Seiki Co., Ltd., a vacuum press manufactured by Mikado Technos, etc.
  • a commercially available vacuum laminating machine such as a vacuum applicator manufactured by Nichigo Morton, a vacuum pressure laminator manufactured by Meiki Seisakusho, a vacuum roll type dry coater manufactured by Hitachi Techno Engineering, or the like It can be manufactured using a belt press or the like.
  • the substrate 10 of the present invention may include a laminate in which the inner circuit board 13 is omitted and the two prepregs 1 are directly bonded to each other, and the metal layer 12 is omitted. It may be what was done.
  • a semiconductor device 100 shown in FIG. 6 connects a bump 501 to the multilayer substrate 200, a pad portion 300 provided on the upper surface of the multilayer substrate 200, a wiring portion 400 provided on the lower surface of the multilayer substrate 200, and the pad portion 300.
  • the semiconductor element 500 mounted on the multilayer substrate 200 is provided.
  • a wiring part, a pad part, a solder ball, and the like may be provided on the lower surface of the multilayer substrate 200.
  • the multilayer substrate 200 includes a substrate 10 provided as a core substrate, three prepregs 1a, 1b and 1c provided on the upper side of the substrate 10, and three prepregs 1d and 1e provided on the lower side of the substrate 10. 1f.
  • the prepregs 1a to 1f are the same as the prepreg 1.
  • the prepregs 1a to 1c are arranged so that the second resin layer 4 is located on the substrate 10 side, that is, in order of the second resin layer 4, the fiber base material 2, and the first resin layer 3 from the substrate 10 side.
  • the prepreg 1 is disposed.
  • the prepregs 1d to 1f are arranged such that the second resin layer 4 is positioned on the substrate 10 side, that is, the second resin layer 4, the fiber base material 2, and the first resin layer 3 are in this order. Is arranged. In the multilayer substrate 200, the resin layers 3 and 4 of the prepreg 1 are completely cured.
  • the multilayer substrate 200 includes a circuit unit 201a provided between the prepreg 1a and the prepreg 1b, a circuit unit 201b provided between the prepreg 1b and the prepreg 1c, and a prepreg 1d and the prepreg 1e.
  • the circuit portion 201d is provided, and the circuit portion 201e is provided between the prepreg 1e and the prepreg 1f.
  • Each of the circuit portions 201 a to 201 e is embedded with the second resin layer 4.
  • the multilayer substrate 200 has holes provided through the respective prepregs 1a to 1f, and in the holes, conductors that electrically connect adjacent circuit parts or circuit parts and pad parts.
  • a portion 202 is formed.
  • Each metal layer 12 of the substrate 10 is processed into a predetermined pattern, and the processed metal layers 12 are electrically connected to each other by a conductor portion 203 provided through the substrate 10.
  • the semiconductor device 100 may include four or more prepregs 1 may be provided on one side of the substrate 10. Furthermore, the semiconductor device 100 may include a prepreg other than the prepreg 1 of the present invention.
  • the present invention is not limited to the above-described embodiment, and modifications, improvements, and the like within the scope that can achieve the object of the present invention are included in the present invention.
  • the prepreg, the substrate, and the semiconductor device of the present invention have been described with respect to the illustrated embodiment.
  • the present invention is not limited to this, and the respective parts constituting the prepreg, the substrate, and the semiconductor device have the same functions. It can be replaced with any configuration that can be exhibited. Moreover, arbitrary components may be added.
  • Appendix 1 A fiber substrate; A first resin layer that covers one surface side of the fiber substrate and is composed of a first resin composition; Covering the other surface side of the fiber substrate, and comprising a second resin layer composed of a second resin composition different from the first resin composition, A prepreg in which the first resin layer and the second resin layer are in contact with each other to form an interface.
  • Appendix 2 In the prepreg described in Appendix 1, The first resin layer is a layer for providing a metal layer on the upper surface thereof, The second resin layer is a prepreg that is a layer for embedding a circuit.
  • the first resin layer protruding from the outer edge of the fiber substrate in plan view and the
  • the total weight of the second resin layer is 5% or less with respect to the total weight of the entire first resin layer and the entire second resin layer, and the rubber plate satisfies the following (i) to (iii): .
  • the first resin layer includes a thermoplastic resin
  • the thermoplastic resin is a prepreg containing at least one of a phenoxy resin, a polyvinyl alcohol resin, and a polyamide resin.
  • the first resin layer and the second resin layer have a naphthalene skeleton, and the prepreg includes an epoxy resin having a structure in which the naphthalene skeleton is bonded to another arylene structure through an oxygen atom.
  • a prepreg produced by impregnating a second resin sheet serving as a second resin layer or a liquid composition containing the second resin composition from the other surface side of the fiber substrate.
  • the second resin layer is a prepreg containing silica having a particle size of 50 nm or less.
  • the fiber base material is a glass cloth, A prepreg in which the silica is present in the strand of the glass cloth.
  • a semiconductor device comprising: a semiconductor element mounted on the substrate.
  • (Appendix 18) Providing a first resin layer made of the first resin composition by pressure-bonding the first resin sheet to one surface of the fiber base; Forming a second resin layer made of a second resin composition different from the first resin composition on the other surface side of the fiber substrate, In the step of forming the second resin layer, The manufacturing method of the prepreg which forms the 2nd resin layer which impregnated the said fiber base material over 90% of the thickness of the said fiber base material from the other surface of the said fiber base material at least. (Appendix 19) In the method for producing a prepreg according to appendix 18, The method for producing a prepreg, wherein the first resin sheet has a minimum melt viscosity at 50 to 150 ° C.
  • Appendix 20 In the method for producing a prepreg according to appendix 18 or 19, In the step of forming the second resin layer, The manufacturing method of the prepreg which supplies a liquid 2nd resin composition to the other surface side of the said fiber base material.
  • Appendix 24 In the method for producing a prepreg according to any one of appendices 18 to 23, The first resin sheet is formed on a support, In the step of pressure-bonding the first resin sheet to one surface of the fiber base material, a prepreg manufacturing method in which the first resin sheet on the support is pressure-bonded to one surface of the fiber base material.
  • Example 1 A first resin composition of A-1 in Table 1 was prepared. First, naphthalene type epoxy resin (Nippon Kayaku Co., Ltd., trade name NC-7300) 12.2 parts by weight, naphthalene type epoxy resin (DIC, trade name HP 4700) 5 parts by weight, phenol novolac type cyanate resin (Lonza) Product name: PT-30) 17.2 parts by weight Biphenyl type phenoxy resin (Mitsubishi Chemical Co., Ltd., trade name YX-6654BH30) 15 parts by weight (in terms of solid content), 1-benzyl-2-methylimidazole as a curing agent ( 0.4 parts by weight of Shikoku Kasei Co., Ltd., Curazole 1B2PZ) was dissolved in methyl ethyl ketone.
  • naphthalene type epoxy resin Nippon Kayaku Co., Ltd., trade name NC-7300
  • DIC naphthalene type epoxy resin
  • an inorganic filler 50 parts by weight of spherical silica (trade name SFP-20M, average particle size 0.3 ⁇ m, manufactured by Denki Kagaku Kogyo Co., Ltd.), epoxy silane coupling agent (trade name KBM-403E, manufactured by Shin-Etsu Chemical Co., Ltd.) ) was added in an amount of 0.2 part by weight and stirred for 60 minutes using a high-speed stirrer. As a result, a varnish of 70% by weight of the resin composition was prepared.
  • spherical silica trade name SFP-20M, average particle size 0.3 ⁇ m, manufactured by Denki Kagaku Kogyo Co., Ltd.
  • epoxy silane coupling agent trade name KBM-403E, manufactured by Shin-Etsu Chemical Co., Ltd.
  • a polyethylene terephthalate film manufactured by Unitika, thickness 38 ⁇ m, width 560 mm
  • the varnish is applied with a comma coater and dried at 170 ° C. for 3 minutes with a drying device, thickness 5 ⁇ m, width 540 mm.
  • the 1st resin sheet (layer used as the 1st resin layer) was formed.
  • the average particle size of silica is determined by measuring the particle size distribution of silica on a volume basis with a dynamic light scattering particle size distribution analyzer (LB-550, manufactured by HORIBA) by dispersing silica in water with ultrasonic waves. The median diameter was defined as the average particle diameter. Specifically, the average particle size is defined by the volume cumulative particle diameter d 50. The same applies to the following examples and comparative examples.
  • a second resin composition having the composition shown in B-1 of Table 2 was prepared. 9 parts by weight of a naphthalene ether type epoxy resin (manufactured by DIC, trade name HP-6000), 6 parts by weight of a biphenyl aralkyl type phenol resin (trade name NC-3000, manufactured by Nippon Kayaku Co., Ltd.), a phenol novolac type cyanate resin (manufactured by Lonza) 15.5 parts by weight of trade name PT-30) was dissolved in methyl ethyl ketone.
  • a naphthalene ether type epoxy resin manufactured by DIC, trade name HP-6000
  • a biphenyl aralkyl type phenol resin trade name NC-3000, manufactured by Nippon Kayaku Co., Ltd.
  • a phenol novolac type cyanate resin manufactured by Lonza
  • inorganic fillers 66 parts by weight of spherical silica (manufactured by Admatechs, SO-31R average particle size 1.0 ⁇ m) and 3 parts by weight of spherical silica (manufactured by Admatechs, trade name Admanano average particle size 50 nm) Then, 0.5 part by weight of an epoxy silane coupling agent (trade name KBM-403E, manufactured by Shin-Etsu Chemical Co., Ltd.) was added, and the mixture was stirred for 60 minutes using a high-speed stirrer. As a result, a varnish of 70% by weight of the resin composition was prepared.
  • an epoxy silane coupling agent trade name KBM-403E, manufactured by Shin-Etsu Chemical Co., Ltd.
  • the varnish containing the second resin composition was discharged from the nozzle 611, and the varnish was supplied to the surface of the fiber base 2 opposite to the first resin layer 3. Then, the varnish containing the first resin sheet 3 ′ and the second resin composition was dried by heating at 120 ° C. for 2 minutes by the drying device 64. Thereby, prepreg 1 (thickness: 35 ⁇ m) was obtained.
  • Example 2 (First resin composition) A first resin composition of A-2 in Table 1 was prepared. First, 12.2 parts by weight of a naphthalene-modified cresol novolak epoxy resin (manufactured by DIC, trade name HP-5000), 5 parts by weight of a naphthalene-type epoxy resin (manufactured by DIC, trade name HP 4700), a phenol novolac-type cyanate resin (Lonza) Product name: PT-30) 17.2 parts by weight Biphenyl type phenoxy resin (Mitsubishi Chemical Co., Ltd., trade name YX-6654BH30) 15 parts by weight (in terms of solid content), 1-benzyl-2-methylimidazole as a curing agent ( 0.4 parts by weight of Shikoku Kasei Co., Ltd., Curazole 1B2PZ) was dissolved in methyl ethyl ketone.
  • a naphthalene-modified cresol novolak epoxy resin manufactured by DIC, trade
  • an inorganic filler 50 parts by weight of spherical fused silica (trade name SFP-20M, average particle size 0.3 ⁇ m, manufactured by Denki Kagaku Kogyo Co., Ltd.), epoxy silane coupling agent (trade name KBM-, manufactured by Shin-Etsu Chemical Co., Ltd.) 403E) was added by 0.2 parts by weight, and the mixture was stirred for 60 minutes using a high-speed stirrer. As a result, a varnish of 70% by weight of the resin composition was prepared.
  • SFP-20M spherical fused silica
  • epoxy silane coupling agent trade name KBM-, manufactured by Shin-Etsu Chemical Co., Ltd.
  • a polyethylene terephthalate film manufactured by Unitika, thickness 38 ⁇ m, width 560 mm
  • the varnish is applied with a comma coater and dried at 170 ° C. for 3 minutes with a drying device, thickness 5 ⁇ m, width 540 mm.
  • the 1st resin sheet (layer used as the 1st resin layer) was formed.
  • Example 2nd resin composition As the 2nd resin composition, the same thing as Example 1 was prepared.
  • Manufacture of prepreg A prepreg was produced in the same manner as in Example 1, using the resin layer with a polyethylene terephthalate film and a varnish containing the second resin composition.
  • DIC naphthalene-modified cresol novolac epoxy resin
  • DIC naphthalene type epoxy resin
  • an inorganic filler 35 parts by weight of spherical fused silica (trade name SFP-20M, average particle size 0.3 ⁇ m, manufactured by Denki Kagaku Kogyo Co., Ltd.), epoxy silane coupling agent (trade name KBM-, manufactured by Shin-Etsu Chemical Co., Ltd.) Then, 0.2 part by weight of 403E) was added and stirred for 60 minutes using a high-speed stirrer. As a result, a varnish of 70% by weight of the resin composition was prepared.
  • SFP-20M spherical fused silica
  • KBM- manufactured by Shin-Etsu Chemical Co., Ltd.
  • a polyethylene terephthalate film (manufactured by Unitika, thickness 38 ⁇ m, width 560 mm) is used as a carrier film, and the varnish is applied with a comma coater and dried at 170 ° C. for 3 minutes with a drying device, thickness 5 ⁇ m, width 540 mm.
  • the 1st resin sheet (layer used as the 1st resin layer) was formed.
  • the 2nd resin composition As the 2nd resin composition, the same thing as Example 1 was prepared.
  • Manufacture of prepreg A prepreg was produced in the same manner as in Example 1, using the resin layer with a polyethylene terephthalate film and a varnish containing the second resin composition.
  • Example 4 (First resin composition) The same 1st resin composition as Example 3 was created, and the same resin layer with a polyethylene terephthalate film as Example 1 was used. (Second resin composition) A second resin composition having the composition shown in B-2 of Table 2 was prepared. 9 parts by weight of dicyclopentadiene type epoxy resin (made by DIC, trade name HP-7200L), 6 parts by weight of biphenyl aralkyl type phenol resin (trade name GPH-65 made by Nippon Kayaku Co., Ltd.), phenol novolac type cyanate resin (Lonza) 15.5 parts by weight of product name PT-30) was dissolved in methyl ethyl ketone.
  • dicyclopentadiene type epoxy resin made by DIC, trade name HP-7200L
  • biphenyl aralkyl type phenol resin trade name GPH-65 made by Nippon Kayaku Co., Ltd.
  • phenol novolac type cyanate resin (Lonza) 15.5 parts by weight of
  • inorganic fillers 66 parts by weight of spherical silica (manufactured by Admatechs, SO-31R average particle diameter 1.0 ⁇ m), 3 parts by weight of spherical fused silica (manufactured by Admatechs, trade name Admanano average particle diameter 50 nm) 0.5 parts by weight of an epoxy silane coupling agent (trade name KBM-403E, manufactured by Shin-Etsu Chemical Co., Ltd.) was added and stirred for 60 minutes using a high-speed stirrer. As a result, a varnish of 70% by weight of the resin composition was prepared.
  • Manufacture of prepreg A prepreg was produced in the same manner as in Example 1 using the resin layer with a polyethylene terephthalate film and the varnish of the second resin composition.
  • Example 5 (First resin composition) The same 1st resin composition as Example 3 was created, and the same resin layer with a polyethylene terephthalate film as Example 1 was used. (Second resin composition) A second resin composition having the composition shown in B-3 of Table 2 was prepared.
  • a naphthalene ether type epoxy resin manufactured by DIC, trade name HP-6000
  • 8 parts by weight of a biphenyl aralkyl type phenol resin trade name GPH-65, manufactured by Nippon Kayaku Co., Ltd.
  • a phenol novolac type cyanate resin manufactured by Lonza 14.5 parts by weight of a trade name PT-30
  • 2 parts by weight (converted to a solid content) of a biphenyl type phenoxy resin (trade name YX-6654BH30, manufactured by Mitsubishi Chemical Corporation) were dissolved in methyl ethyl ketone.
  • Example 6 (First resin composition) The same 1st resin composition as Example 3 was created, and the same resin layer with a polyethylene terephthalate film as Example 1 was used. (Second resin composition) A second resin composition having the composition shown in B-2 of Table 2 was prepared.
  • a prepreg was produced using the varnish of the first resin composition having the composition of A-1 produced in Example 1 and the varnish of the second resin composition having the composition represented by B-1.
  • a die coater was used from both sides of the fiber base, and the varnish of the first resin composition was applied to one side, and the varnish of the second resin composition was applied to the other side, and dried by heating at 180 ° C. for 2 minutes. Thereby, a prepreg (thickness: 35 ⁇ m) was obtained.
  • Example 2 the prepreg was manufactured by the method similar to Example 1 of the pamphlet of international publication WO2007 / 063960. Details are as follows. 1. Preparation of first resin layer varnish Cyanate resin (Lonza Japan, Primaset PT-30, weight average molecular weight about 2,600) 24% by weight, biphenyldimethylene type epoxy resin (manufactured by Nippon Kayaku Co., Ltd.) NC-3000, epoxy equivalent 275) 24% by weight, phenoxy resin is a copolymer of bisphenol A type epoxy resin and bisphenol F type epoxy resin, and the terminal part is a phenoxy resin having an epoxy group (Japan epoxy resin) 11.8% by weight, EP-4275, weight average molecular weight 60,000), 0.2 weight by weight of imidazole compound as a curing catalyst (“2-phenyl-4,5-dihydroxymethylimidazole” manufactured by Shikoku Chemicals) % Was dissolved in methyl ethyl ketone.
  • Cyanate resin Lionza Japan
  • composition A-4 in Table 3 39.8% by weight of spherical fused silica (manufactured by Admatechs, SO-25H, average particle size 0.5 ⁇ m) as an inorganic filler and epoxy silane type coupling agent (manufactured by Nihon Unicar, A-187) 0. 2% by weight was added and stirred for 60 minutes using a high-speed stirrer to prepare a resin varnish of 70% by weight of the resin composition (composition A-4 in Table 3).
  • spherical fused silica manufactured by Admatechs, SO-25H, average particle size 0.5 ⁇ m
  • epoxy silane type coupling agent manufactured by Nihon Unicar, A-187
  • varnish of second resin layer 15% by weight of novolak-type cyanate resin (manufactured by Lonza Japan, Primaset PT-30, weight average molecular weight of about 2,600) as thermosetting resin, biphenyldimethylene type epoxy resin as epoxy resin (Nippon Kayaku Co., Ltd., NC-3000, epoxy equivalent 275) 8.7% by weight, phenol resin biphenyldimethylene type phenol resin (Nippon Kayaku Co., Ltd., GPH-65, hydroxyl equivalent 200) 6.3% by weight Was dissolved in methyl ethyl ketone.
  • novolak-type cyanate resin manufactured by Lonza Japan, Primaset PT-30, weight average molecular weight of about 2,600
  • biphenyldimethylene type epoxy resin as epoxy resin
  • phenol resin biphenyldimethylene type phenol resin Nippon Kayaku Co., Ltd., GPH-65, hydroxyl equivalent 200
  • spherical fused silica manufactured by Admatechs, SO-25H, average particle size 0.5 ⁇ m
  • inorganic filler 69.7% by weight
  • epoxysilane type coupling agent Nihon Unicar Co., Ltd., A-187 0. 3% by weight was added, and the mixture was stirred for 60 minutes using a high-speed stirrer to prepare a varnish for the second resin layer of 70% by weight of the resin composition (composition B-5 in Table 3).
  • carrier material A polyethylene terephthalate film (manufactured by Mitsubishi Chemical Polyester Co., Ltd., SFB-38, thickness 38 ⁇ mm, width 480 mm) was used as a carrier film.
  • the carrier material I finally the first resin layer is finally formed
  • the carrier material I is formed by drying for 3 minutes using a drying apparatus and forming a resin layer having a thickness of 9 ⁇ m and a width of 410 mm at the center in the width direction of the carrier film. Obtained.
  • the amount of the varnish of the second resin layer to be coated by the same method is adjusted so that the resin layer having a thickness of 14 ⁇ m and a width of 360 mm is positioned at the center in the width direction of the carrier film.
  • II final formation of the second resin layer
  • Prepreg Glass woven fabric cross type # 1015, width 360 mm, thickness 15 ⁇ m, basis weight 17 g / m 2
  • a prepreg was produced by a vacuum laminating apparatus and a hot air drying apparatus.
  • the carrier material I and the carrier material II are overlapped on both surfaces of the glass woven fabric so as to be positioned at the center in the width direction of the glass woven fabric, respectively, and are laminated at 80 ° C. under a reduced pressure of 1330 Pa. Was used for bonding.
  • the resin layers of the carrier material I and the carrier material II are respectively bonded to both sides of the fiber cloth, and in the outer region of the width direction dimension of the glass woven fabric.
  • the resin layers of carrier material I and carrier material II were joined together.
  • the bonded material was heat-treated without applying pressure by passing it through a horizontal conveyance type hot-air drying apparatus set at 120 ° C. for 2 minutes to obtain a thickness of 30 ⁇ m (first resin layer: 5 ⁇ m, A prepreg having a fiber base material of 15 ⁇ m and a second resin layer of 10 ⁇ m was obtained.
  • the peel strength of the first resin layer and the second resin layer of each of the examples and comparative examples was measured.
  • the measuring method is as follows.
  • the first resin layer 3 of the prepreg 1 was placed on a copper foil, and the 90 ° peel strength A after heat treatment in the atmosphere under the conditions of a load of 2 MPa, a temperature of 220 ° C. and 1 hour was measured.
  • the second resin layer 4 of the prepreg was placed on a copper foil, and the 90 ° peel strength B after heat treatment in the atmosphere under the conditions of a load of 2 MPa, a temperature of 220 ° C. and 1 hour was measured.
  • the peel strength was measured in accordance with JIS C 6481 90 degree peeling method by peeling the resin layer from the copper foil in the 90 degree direction. Specifically, at 25 ° C., the 90 ° peel strength when the resin layer was peeled off at a speed of 50 mm per minute was measured with a 90 ° peel tester.
  • a prepreg was stacked so that the second resin layer was in contact with the circuit pattern of the inner layer circuit board, and pressure heating molding (1 MPa, 200 ° C., 90 minutes) was performed to obtain 10 substrates. The cross section of each substrate was observed with a microscope. Then, the embedding property of the second resin layer was evaluated. (Double-circle): It was excellent in the embedding property in all the board
  • the measurement conditions for the minimum melt viscosity are as follows. The results are shown in Table 4. In Examples and Comparative Examples, the lowest melt viscosities of the first resin layer and the second resin layer at 50 to 150 ° C. were measured. Here, the varnish of the first resin composition and the varnish of the second resin composition obtained in the respective Examples and Comparative Examples were applied with a comma coater device, dried at 170 ° C. for 3 minutes with a drying device, and a thickness of 5 ⁇ m. The film is a measurement object. However, the measurement result here corresponds to the minimum melt viscosity of the first resin layer and the second resin layer in the prepreg state. The measurement conditions are as follows.
  • Dynamic viscoelasticity measuring device manufactured by Anton Paar, device name Physica MCR-301
  • Frequency 62.83 rad / sec
  • Measurement temperature 25-200 ° C, 3 ° C / min
  • Geometry Parallel plate Plate diameter: 10mm Plate spacing: 0.1mm
  • Measurement atmosphere Air
  • the prepregs of Examples and Comparative Examples cut to 200 mm ⁇ 200 mm were pressed using a hot press device of CVP300 manufactured by Nichigo-Morton Co., Ltd., and the amount of resin protrusion was measured. Specifically, the prepreg of the above example or comparative example is placed between two rubber plates sandwiched between two hot plates (SUS 1.5 mm) of this hot press apparatus, and the conditions are 120 ° C. and 2.5 MPa. And pressed for 60 seconds.
  • the rubber plate was a silicon rubber having a rubber hardness measured according to JIS K 6253 A of 60 ° and a thickness of 3 mm. The results are shown in Table 4.
  • the laminated body is pre-dried at 125 ° C./24 hours, then subjected to moisture absorption treatment at 85 ° C. and 60% 196 hours, and reflow for lead-free solder having a peak temperature of 260 ° C.
  • the profile infrared reflow oven was passed 20 times. At each reflow, the appearance of the laminate was observed to confirm the presence or absence of swelling.
  • the swelling inside the laminate was also investigated using SAT (ultrasonic imaging device). The results are shown in Table 4. (Double-circle): There is no swelling of an external appearance after passing 20 times of reflow ovens. No swelling inside the laminate. ⁇ : No swelling of the appearance after passing through the reflow furnace 20 times. There is swelling inside the laminate. ⁇ : Appearance swelled after passing through the reflow furnace 1 to 5 times.
  • the peel strength A of the first resin layer is higher than the peel strength B of the second resin layer, and the peel strength of the first resin layer and the second resin layer becomes the desired strength.
  • the embedding property of the circuit pattern is also good, and it can be seen that the first resin layer and the second resin layer can exhibit desired characteristics. Further, it can be seen that the resin flow is 15% by weight or more, and the circuit embedding property is excellent. Further, the resin flow was 50% by weight or less, and the outflow of the resin during pressing could be suppressed. Moreover, since the protrusion amount of resin is 5 weight% or less, the thickness uniformity of a laminated board is favorable and generation
  • the heat resistance is very good because silica having an average particle diameter of 50 nm is used for the second resin layer.
  • the reliability between vias is very high because silica having an average particle diameter of 50 nm is used for the second resin layer. It is considered that the reliability between vias is improved when nanosilica enters the fiber bundle and nanosilica adheres to the fiber.
  • the prepreg using the naphthylene ether type epoxy resin had low water absorption and low thermal expansion.
  • Comparative Example 1 since the fiber base material is impregnated with the varnish having the same degree of viscosity, the impregnation rates of the first resin layer and the second resin layer are the same, and the impregnation rate is considered to be about 50%. . Furthermore, in Comparative Example 2, since the resin sheets having very close minimum melt viscosities are bonded to the fiber base material, the impregnation rates of the first resin layer and the second resin layer are approximately the same, and the impregnation rate is approximately 50%. It is thought that. In such Comparative Examples 1 and 2, since it is necessary to impregnate the fiber base material to the same extent with the first resin layer and the second resin layer, the selection of the resin composition is limited.
  • Comparative Example 1 the interface between the first resin layer and the second resin layer cannot be confirmed, and the first resin layer and the second resin layer are mixed. Therefore, the peel strength of the first resin layer is weaker than that of Example 1. Furthermore, the embedding property of the circuit pattern is inferior to that of Example 1, and the first resin layer and the second resin layer cannot exhibit desired characteristics. Furthermore, the reliability between vias is poor, the thickness uniformity of the laminate is poor, and warping occurs. In Comparative Example 1, the point that the reliability between vias is poor is considered to be due to the non-uniform mixing of the varnish constituting the first resin layer and the varnish constituting the second resin layer.
  • Comparative Example 2 the interface between the first resin layer and the second resin layer cannot be confirmed, and the first resin layer and the second resin layer are mixed. Therefore, the peel strength of the first resin layer is lower than the desired value. Further, in Comparative Example 2, warpage occurs in the laminated plate. This is because the first resin layer on the copper foil side has a low viscosity, and thus the thickness of the laminated plate varies.

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